Atomic Efficient Catalytic Technology for Sustainable Chemical and Fuel Syntheses Enabled by Active Site Coupling and Kinetic Property Tuning

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Efficient synthesis of energy carriers and commodity, specialty, and pharmaceutical chemicals from renewable feedstocks is one of the greatest challenges of this century, paving the path towards a sustainable future. The proposed research program will develop fundamental catalytic knowledge required for this synthesis via the design of catalytic sites and reaction environments and, in turn, tuning of rates and selectivities in order to attain the much sought after atomistic efficiencies. The specific research themes are the conversion of light alkanes, selective hydrogenation of aldehydes/ketones, and coupling of light oxygenates from alternative feedstocks (shale gas, biogas, and lignocellulosic biomass). The program will adapt a highly integrated, multidisciplinary approach, combining advanced spectroscopic and microscopic techniques, density functional theory, together with kinetic and isotopic transient methods, to unravel the catalytic events at the molecular scale. Specific focus is on the structural dynamics of active sites upon their contact with complex solvent mixtures and the instantaneous formation of active structures during catalysis under industrially relevant conditions. Our previous work has established the kinetic functions of well-defined metal and Brønsted acid sites and the catalytic requirements for these reactions with great molecular details. We have also identified key kinetic descriptors, i.e., measurable thermodynamic properties, that dictate the fate of the reactants during their catalytic sojourns. In this next phase, we will exploit the mechanistic knowledge and catalytic requirements, in designing complex, hierarchical catalyst structures with multiple types of mono-functional sites, containing them in confined structures and altering their reaction environment with aggregated solvent molecules for atomic efficient catalysis. Such strategies alter the chemical identity and reactivity of the intermediates and, in turn, dictate the ultimate yields. Incorporating into this program is a comprehensive professional development plan, placing strong emphasis on diverse, interdisciplinary trainings across chemical engineering, chemistry, materials science, as well as on critical thinking and leadership competency. The highly qualified personnel trained from this program will acquire strong technical and professional skill sets with broad industrial and global perspective, through strong, synergistic collaborative efforts and the use of world class infrastructure, within Canada as well as in the US. The personnel will work on fundamental problems, directly transferrable to those in industrial catalysis, as such they are much needed in the Canadian energy and chemical industries.